Cellulose nanocrystals (CNCs) are promising renewable nanoparticles with unique properties including high mechanical strength and a large aspect ratio. As such, CNCs easily form strong gels and networked structures. “Entangled” CNC systems generally rely on physical cross-links however we demonstrate the chemical cross-linking of CNCs through hydrazone bonds. CNCs functionalized with dihydrazide groups and aldehyde groups covalently cross-link instantly when they come into contact. Cross-linked CNC aerogels possess some of the lowest reported densities to-date, are strong and can absorb 70-160 times their weight in both water and non-polar solvents, without disintegrating. Furthermore, they can recover their shape by 85% after being compressed over 80%. These aerogels make extraordinary scaffolds and templates to support other materials. We demonstrate the incorporation of conductive polymers, carbon nanotubes, inorganic nanoparticles, core-shell polymer latexes, and metal organic frameworks into CNC aerogels. Various routes to incorporate conductive materials and nanoparticles are investigated including in situ “trapping” during aerogel preparation, back-filling, and a “polymerizing-from aerogel” approach. Combining CNCs and functional nanoparticles leads to strong, flexible, and free-standing devices with applications as supercapacitors, water purification systems and adsorbents.

Cross-linked cellulose nanocrystal aerogels as universal 3D substrates for functional nanoparticles

251st National Meeting (2016)

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